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Water Environment Research : a Research... May 2024Photocatalytic oxidation-adsorption synergistic treatment of organic arsenic pollutants is a promising wastewater treatment technology, which not only degrades organic... (Review)
Review
Photocatalytic oxidation-adsorption synergistic treatment of organic arsenic pollutants is a promising wastewater treatment technology, which not only degrades organic arsenic pollutants by photocatalytic degradation but also removes the generated inorganic arsenic by adsorption. This paper compares the results of photocatalytic oxidation-adsorption co-treatment of organic arsenic pollutants such as monomethylarsonic acid, dimethylarsinic acid, phenylarsonic acid, p-arsanilic acid, and 3-nitro-4-hydroxyphenylarsonic acid on titanium dioxide, goethite, zinc oxide, and copper oxide. It examines the influence of the morphology of organic arsenic molecules, pH, coexisting ions, and the role of natural organic matter. The photocatalytic oxidation-adsorption co-treatment mechanism is investigated, comparing the hydroxyl radical oxidation mechanism, the hydroxyl radical and superoxide anion radical cooxidation mechanism, and the hydroxyl radical and hole cooxidation mechanism. Finally, the future prospects of metal oxide photocatalytic materials and the development of robust and efficient technologies for removing organic arsenic are envisioned.
Topics: Water Pollutants, Chemical; Oxidation-Reduction; Adsorption; Catalysis; Water Purification; Arsenic; Photochemical Processes
PubMed: 38797515
DOI: 10.1002/wer.11057 -
Materials (Basel, Switzerland) Dec 2023As a kind of emerging contaminant, organoarsenic compounds have drawn wide concern because of their considerable solubilities in water, and the highly toxic inorganic...
As a kind of emerging contaminant, organoarsenic compounds have drawn wide concern because of their considerable solubilities in water, and the highly toxic inorganic arsenic species formed during their biotic and abiotic degradation in the natural environment. Thus, the effective removal and studying of the adsorption mechanism of organoarsenic compounds are of significant urgency. In this work, MnFeO and MnFeO/graphene were prepared through a facile solvothermal method. From the results of the Transmission Electron Microscope (TEM) characterization, it can be found that MnFeO nanoparticles were uniformly distributed on the surface of the graphene. And the specific surface area of the MnFeO/graphene was about 146.39 m g, much higher than that of the MnFeO (86.15 m g). The interactions between organoarsenic compounds and adsorbents were conducted to study their adsorption behavior and mechanism. The maximum adsorption capacities of MnFeO/graphene towards p-arsanilic acid (p-ASA) and roxarsone (ROX) were calculated to be 22.75 and 30.59 mg g. Additionally, the ionic strength, negative ions, and humus were introduced to investigate the adsorption performance of organoarsenic compounds. Electrostatic adsorption and surface complexation are the primary adsorption mechanisms on account of X-ray photoelectron spectroscopy (XPS) and the Fourier-transform infrared spectroscopy (FT-IR) analysis. This research extends the knowledge into studying the interaction between organoarsenic species and hybrid nanomaterials in the natural environment.
PubMed: 38138778
DOI: 10.3390/ma16247636 -
Water Research Feb 2024As a widely used feed additives, p-arsanilic acid (p-AsA) frequently detected in the environment poses serious threats to aquatic ecology and water security due to its...
Comparative study of Fe(II)/sulfite, Fe(II)/PDS and Fe(II)/PMS for p-arsanilic acid treatment: Efficient organic arsenic degradation and contrasting total arsenic removal.
As a widely used feed additives, p-arsanilic acid (p-AsA) frequently detected in the environment poses serious threats to aquatic ecology and water security due to its potential in releasing more toxic inorganic arsenic. In this work, the efficiency of Fe(II)/sulfite, Fe(II)/PDS and Fe(II)/PMS systems in p-AsA degradation and simultaneous arsenic removal was comparatively investigated for the first time. Efficient p-AsA abatement was achieved in theses Fe-based systems, while notable discrepancy in total arsenic removal was observed under identical acidic condition. By using chemical probing method, quenching experiments, isotopically labeled water experiments, p-AsA degradation was ascribed to the combined contribution of high-valent Fe(IV) and SOin these Fe(II)-based system. In particular, the relative contribution of Fe(IV) and SO in the Fe(II)/sulfite system was highly dependent on the molar ratio of [Fe(II)] and [sulfite]. Negligible arsenic removal was observed in the Fe(II)/sulfite and Fe(II)/PDS systems, while ∼80% arsenic was removed in the Fe(II)/PMS system under identical acidic condition. This interesting phenomenon was due to that ferric precipitation only occurred in the Fe(II)/PMS system. As(V) was further removed via adsorption onto the iron precipitate or the formation of ferric arsenate-sulfate compounds, which was confirmed by particle diameter measurements, fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. Through tuning solution pH, complete removal of total arsenic could achieve in all three systems. Among these three Fe-based technologies, the hybrid oxidation-coagulation Fe(II)/PMS system demonstrated potential superiority for arsenic immobilization by not requiring pH adjustment for coagulation and facilitating the in-situ generation of ferric arsenate-sulfate compounds with comparably low solubility levels like scorodite. These findings would deepen the understanding of these three Fe-based Fenton-like technologies for decontamination in water treatment.
Topics: Arsenic; Arsenates; Arsanilic Acid; Iron; Ferric Compounds; Oxidation-Reduction; Sulfites; Sulfates; Sulfur Oxides; Ferrous Compounds; Water Pollutants, Chemical
PubMed: 38070343
DOI: 10.1016/j.watres.2023.120967 -
Environmental Research Mar 2024Arsanilic acid (p-AsA), a prevalently used feed additive, is frequently detected in environment posing a great threat to humans. Potassium ferrate (Fe(VI)) was an...
Arsanilic acid (p-AsA), a prevalently used feed additive, is frequently detected in environment posing a great threat to humans. Potassium ferrate (Fe(VI)) was an efficient way to tackle arsenic contamination under acid and neutral conditions. However, Fe(VI) showed a noneffective removal of p-AsA under alkaline conditions due to its oxidation capacity attenuation. Herein, a magnetic iron-doped carbon nanotubes (F-CNT) was successfully prepared and further catalyzed Fe(VI) to remove p-AsA and total As species. The Fe(VI)/F-CNT system showed an excellent capability to oxidize p-AsA and adsorb total As species over an environment-related pH range of 6-9. The high-valent iron intermediates Fe(V)/Fe(IV) and the mediated electron-transfer played a significant part in the degradation of p-AsA according to the probes/scavengers experiments and galvanic oxidation process. Moreover, the situ formed iron hydroxide oxide and F-CNT significantly improved the adsorption capacity for total As species. The electron-donating groups (semiquinone and hydroquinone) and high graphitization of F-CNT were responsible for activating Fe(VI) based on the analysis of X-ray photoelectron spectroscopy (XPS). Density functional theory calculations and the detected degradation products both indicated that the amino group and the C-As bond of p-AsA were main reactive sites. Notably, Fe(VI)/F-CNT system was resistant to the interference from Cl, SO, and HCO, and could effectively remove p-AsA and total As species even in the presence of complex water matrix. In summary, this work proposed an efficient method to use Fe(VI) for degrading pollutants under alkaline conditions and explore a new technology for livestock wastewater advanced treatment.
Topics: Humans; Iron; Nanotubes, Carbon; Arsanilic Acid; Arsenic; Electrons; Oxidation-Reduction; Water Pollutants, Chemical; Water Purification; Ferric Compounds
PubMed: 38061591
DOI: 10.1016/j.envres.2023.117849 -
Journal of Hazardous Materials Feb 2024Aromatic organoarsenic feed additives have been extensively used in poultry and livestock farming; however, a risk of releasing toxic inorganic arsenic exists when they...
Aromatic organoarsenic feed additives have been extensively used in poultry and livestock farming; however, a risk of releasing toxic inorganic arsenic exists when they are exposed to the environment. An in-depth understanding of the adsorption -migration behavior of aromatic organoarsenicals on environmental media is limited. In this study, p-arsanilic acid (p-ASA) and roxarsone (ROX) were considered as examples to systematically study their adsorption behaviors on the surface of hematite, a representative iron oxide in soil. By comparing the adsorption abilities and adsorption kinetics of hematite exposed with different facets (hexagonal nanoplates, HNPs, mainly exposed with {001} facets and hexagonal nanocubes, HNCs, exposed with {012} facets), combined with in situ shell-isolated nanoparticle enhanced Raman spectroscopy characterization and density functional theory simulation, the facet-dependent adsorption performance was observed and the mechanism revealed. The results showed that p-ASA formed a bidentate binuclear complex on HNCs and HNPs, whereas ROX formed monodentate mononuclear and bidentate binuclear configurations on the {001} and {012} facets, respectively. These differences not only lead to facet-dependent adsorption capacities but also affect their stability, as verified by sequential extraction experiments, affecting the environmental behavior and fate of aromatic organoarsenicals. This study not only provides insights into the environmental behavior of aromatic organoarsenicals but also offers theoretical support for the development of functional adsorbents and remediation strategies.
PubMed: 37976861
DOI: 10.1016/j.jhazmat.2023.132976 -
Chemosphere Dec 2023Roxarsone (3-nitro-4-hydroxyphenylarsonic acid, Rox), a widely used organoarsenical feed additive, can enter soils and be further biotransformed into various arsenic...
Roxarsone (3-nitro-4-hydroxyphenylarsonic acid, Rox), a widely used organoarsenical feed additive, can enter soils and be further biotransformed into various arsenic species that pose human health and ecological risks. However, the pathway and molecular mechanism of Rox biotransformation by soil microbes are not well studied. Therefore, in this study, we isolated a Rox-transforming bacterium from manure-fertilized soil and identified it as Pseudomonas chlororaphis through morphological analysis and 16S rRNA gene sequencing. Pseudomonas chlororaphis was able to biotransform Rox to 3-amino-4-hydroxyphenylarsonic acid (3-AHPAA), N-acetyl-4-hydroxy-m-arsanilic acid (N-AHPAA), arsenate [As(V)], arsenite [As(III)], and dimethylarsenate [DMAs(V)]. The complete genome of Pseudomonas chlororaphis was sequenced. PcmdaB, encoding a nitroreductase, and PcnhoA, encoding an acetyltransferase, were identified in the genome of Pseudomonas chlororaphis. Expression of PcmdaB and PcnhoA in E. coli Rosetta was shown to confer Rox(III) and 3-AHPAA(III) resistance through Rox nitroreduction and 3-AHPAA acetylation, respectively. The PcMdaB and PcNhoA enzymes were further purified and functionally characterized in vitro. The kinetic data of both PcMdaB and PcNhoA were well fit to the Michaelis-Menten equation, and nitroreduction catalyzed by PcMdaB is the rate-limiting step for Rox transformation. Our results provide new insights into the environmental risk assessment and bioremediation of Rox(V)-contaminated soils.
Topics: Humans; Roxarsone; Pseudomonas chlororaphis; Soil; Acetyltransferases; RNA, Ribosomal, 16S; Escherichia coli; Arsenic; Biotransformation; Nitroreductases
PubMed: 37898462
DOI: 10.1016/j.chemosphere.2023.140558 -
ACS Applied Materials & Interfaces Oct 2023Metal-organic frameworks (MOFs) are emerging as advanced nanoporous materials to remove phenylarsenic acid, -arsanilic acid (-ASA), and roxarsone (ROX) in the aqueous...
Metal-organic frameworks (MOFs) are emerging as advanced nanoporous materials to remove phenylarsenic acid, -arsanilic acid (-ASA), and roxarsone (ROX) in the aqueous solution, while MOFs are often present as powder state and encounter difficulties in recovery after adsorption, which greatly limit their practical application in the aqueous environments. Herein, MIL-101 (Fe), a typical MOF, was mixed with sodium alginate and gelatin to prepare MIL-101@CAGE by three-dimensional (3D) printing technology, which was then used as a separatable adsorbent to remove phenylarsenic acid in the aqueous solution. The structure of 3D-printed MIL-101@CAGE was first characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FTIR), and thermogravimetry and differential thermogravimetry (TG-DTG). The octahedral morphology of MIL-101 (Fe) was found unchanged during the 3D printing process. Then, the adsorption process of MIL-101@CAGE on phenylarsenic acids was systematically investigated by adsorption kinetics, adsorption isotherms, adsorption thermodynamics, condition experiments, and cyclic regeneration experiments. Finally, the adsorption mechanism between MIL-101@CAGE and phenylarsenic acid was further investigated. The results showed that the Langmuir, Freundlich, and Temkin isotherms were well fit, and according to the Langmuir fitting results, the maximum adsorption amounts of MIL-101@CAGE on -ASA and ROX at 25 °C were 106.98 and 120.28 mg/g, respectively. The removal of -ASA and ROX by MIL-101@CAGE remained stable over a wide pH range and in the presence of various coexisting ions. The regeneration experiments showed that the 3D-printed MIL-101@CAGE could still maintain a more than 90% removal rate after five cycles. The adsorption mechanism of this system might include π-π stacking interactions between the benzene ring on the phenylarsenic acids and the organic ligands in MIL-101@CAGE, hydrogen-bonding, and ligand-bonding interactions (Fe-O-As). This study provides a new idea for the scale preparation of a separatable and recyclable adsorbent based on MOF material for the efficient removal of phenylarsenic acid in the aqueous solution.
PubMed: 37816194
DOI: 10.1021/acsami.3c10766 -
The Science of the Total Environment Jan 2024Although banned in some countries, p-arsanilic acid (ASA) is still widely used as feed additive in poultry production. As a result, ASA is usually released into the...
Although banned in some countries, p-arsanilic acid (ASA) is still widely used as feed additive in poultry production. As a result, ASA is usually released into the aquatic environment without any treatments. Although ASA exhibits low toxicity, it can be transformed into highly toxic aromatic amines and inorganic arsenic species (As (V) as HAsO and HAsO) under natural environmental conditions. Hence, it is necessary to develop efficient technologies for its removal or degradation. In this contribution, electrochemical advanced oxidation technology with boron-doped diamond (BDD) had been initially used to degrade ASA pollutants. A five-level central composite rotatable design (CCRD) was implemented to optimize the various influencing factors involved, among applied current density, NaCl concentration, NaSO concentration and NaHCO concentration on the oxidation efficiency; the latter was assessed in terms of ASA degradation percentage. The results obtained highlighted the unique and important roles of electrolytes during the electrolytic oxidations. Meanwhile, the major degradation byproducts detected were also strongly dependent on the electrolyte adopted. In particular, several oligomer byproducts with novel structures were initially identified in BDD-treated ASA solutions. Two different electrochemical transformation pathways of ASA on BDD anode were thus proposed. This study demonstrated the effectiveness of BDD technology in the degradation of ASA, as well as the potential minor risk of its application in actual ASA wastewater treatment.
PubMed: 37797755
DOI: 10.1016/j.scitotenv.2023.167538 -
Environmental Science and Pollution... May 2024The widespread used organoarsenicals have drawn attention for decades due to their potential environment risks. In this study, a heterogeneous system of goethite/oxalate...
The widespread used organoarsenicals have drawn attention for decades due to their potential environment risks. In this study, a heterogeneous system of goethite/oxalate irradiated using UVA light (λ = 365 nm) was applied for the removal of ASA, a kind of organoarsenicals used in animal feeding operations as additives, from the aqueous phase through photodegradation. Results showed that the presence of 5 mM of oxalate significantly enhanced the photodegradation efficiency of ASA in the 0.1 g/L of goethite suspended system from 28 to ~100% within 180 min reaction at pH 5. Acid conditions favored the photoreaction rate, compared with neutral and basic conditions. This reaction process was also influenced by the initial concentration of oxalate and ASA. Furthermore, the mechanism study was conducted by quenching experiments and revealed the important roles of ·OH in the degradation of ASA in the goethite/oxalate/UVA system. By analyzing the reaction products, both inorganic arsenic (As(III) and As(V)) and ammonia were detected during the photodegradation of ASA. These findings help to gain a better understanding of the geochemical behavior of ASA in surface water and can also provide a potential treatment method for the organoarsenicals contaminated water.
Topics: Ultraviolet Rays; Oxalates; Photolysis; Minerals; Iron Compounds; Arsanilic Acid; Water Pollutants, Chemical
PubMed: 37594713
DOI: 10.1007/s11356-023-29289-9 -
Frontiers in Neurology 2023Betahistine is widely used for the treatment of various vestibular disorders. However, the approved oral administration route and maximum daily dose are evidently not...
INTRODUCTION
Betahistine is widely used for the treatment of various vestibular disorders. However, the approved oral administration route and maximum daily dose are evidently not effective in clinical trials, possibly due to a major first-pass metabolism by monoamine oxidases (MAOs). The current study aimed to test different application routes (i.v./s.c./p.o.), doses, and concurrent medication (with the MAO-B inhibitor selegiline) for their effects on behavioral recovery and cerebral target engagement following unilateral labyrinthectomy (UL) in rats.
METHODS
Sixty rats were subjected to UL by transtympanic injection of bupivacaine/arsanilic acid and assigned to five treatment groups: i.v. low-dose betahistine (1 mg/kg bid), i.v. high-dose betahistine (10 mg/kg bid), p.o. betahistine (1 mg/kg bid)/selegiline (1 mg/kg once daily), s.c. betahistine (continuous release of 4.8 mg/day), and i.v. normal saline bid (sham treatment; days 1-3 post-UL), respectively. Behavioral testing of postural asymmetry, nystagmus, and mobility in an open field was performed seven times until day 30 post-UL and paralleled by sequential cerebral [F]-FDG-μPET measurements.
RESULTS
The therapeutic effects of betahistine after UL differed in extent and time course and were dependent on the dose, application route, and selegiline co-medication: Postural asymmetry was significantly reduced on 2-3 days post-UL by i.v. high-dose and s.c. betahistine only. No changes were observed in the intensity of nystagmus across groups. When compared to sham treatment, movement distance in the open field increased up to 5-fold from 2 to 30 days post-UL in the s.c., i.v. high-dose, and p.o. betahistine/selegiline groups. [F]-FDG-μPET showed a dose-dependent rCGM increase in the ipsilesional vestibular nucleus until day 3 post-UL for i.v. high- vs. low-dose betahistine and sham treatment, as well as for p.o. betahistine/selegiline and s.c. betahistine vs. sham treatment. From 1 to 30 days post-UL, rCGM increased in the thalamus bilaterally for i.v. high-dose betahistine, s.c. betahistine, and p.o. betahistine/selegiline vs. saline treatment.
DISCUSSION
Betahistine has the potential to augment the recovery of dynamic deficits after UL if the administration protocol is optimized toward higher effective plasma levels. This may be achieved by higher doses, inhibition of MAO-based metabolism, or a parenteral route. imaging suggests a drug-target engagement in central vestibular networks.
PubMed: 37538257
DOI: 10.3389/fneur.2023.1175481